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Like the ship's other junior officers, Lowe reported to White Star's Liverpool offices at nine o'clock in the morning on 26 March 1912, and travelled to board the Titanic at Belfast the following day. On sailing day (10 April), Lowe assisted (among other things) in the lowering of two of the starboard lifeboats to satisfy the Board of Trade that the Titanic met safety regulations. When the Titanic departed Southampton at noon, Lowe was on the bridge, relaying messages to various parts of the ship by telephone.

On 14 April 1912, the night of the sinking, Lowe had been relieved at 8.00 PM by Sixth Officer Moody and was asleep in his quarters when the ship hit the iceberg at 11.40 PM. He remained asleep through the collision and did not wake up until as much as half an hour had passed; as he explained later, "We officers do not have any too much sleep, and therefore when we sleep, we die." When Lowe finally awakened and realised the situation, he immediately got dressed, grabbed his revolver, and went to work. Third Officer Pitman charged him with loading lifeboat No. 5. Around 1.30 AM, Lowe engaged in a conversation with Sixth Officer Moody: While launching lifeboat Nos. 14 and 16 on the port side of the ship, the two junior officers felt that this group of boats needed to have an officer with them. Moody insisted that Lowe should get onto lifeboat No. 14 and that he would get on another one. By the time lifeboat 14 was being launched, things were beginning to get precarious on the boat deck as the majority of passengers began to realise that the giant ship was foundering. As lifeboat 14 was descending, Lowe used his pistol to fire three warning shots parallel to the ship in order to frighten away a group of men attempting to leap into the lifeboat.

Harold Lowe attempting to rescue any survivors from the Titanic.

After reaching the water, Lowe ordered his lifeboat to be rowed about 150 yd (140 m) away from the Titanic. When the ship foundered at around 2.20 AM, Lowe had begun to gather several lifeboats together. These were lifeboats 4,10,12,14, and Collapsible D. He wished to return to pick up survivors but had fears of being swamped by hordes of people. He redistributed the survivors in the group of lifeboats he had gathered, to ready his boat, number 14, for a search to find additional survivors. The lifeboat he took back to the site of the sinking had no passengers and an excess of crewmen, saying "Is there anyone alive out there" to facilitate rescue. Reluctantly, he waited until the screams died down before returning. When he returned to gather survivors, he picked up only four men. One of them, 1st class passenger W.F. Hoyt, later died that night. Lowe's was the only boat to return for survivors. After that, Lowe had his crew of men raise the mast (he was the only officer to make use of the mast and sail in each lifeboat); using a breeze that had sprung up, he continued on to rescue the passengers on the sinking Collapsible A. Certain that the swamped collapsible would sink in minutes, Lowe left two dead men aboard this boat where they were, covering their faces with lifebelts. A month later, Collapsible A was discovered still afloat -some 200 miles from the sinking- by the RMS Oceanic, with the two dead men still aboard just as Lowe had left them. Lowe and his group of lifeboats were picked up the next morning by the RMS Carpathia. An image taken by a passenger on the Carpathia clearly shows Lowe at the tiller of Lifeboat 14 as they approach rescue. He remained aboard his lifeboat long enough to ship the mast and make certain everything was properly stowed.

He is seen later rescuing Rose DeWitt Bukater from the freezing water and summoning the RMS Carpathia by lighting and waving the flares. In a deleted scene, he appears helping Rose onboard to safety.